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1.
Mater Horiz ; 2024 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-39315763

RESUMO

Circularly polarized phosphorescent (CPP) materials, especially chiral platinum(II) complexes, which combine the advantages of both circularly polarized luminescence (CPL) and phosphorescence, show broad potential applications in chiral optoelectronic devices. Developing CPP emitters with both excellent chiroptical properties and high yield is urgently needed. Here, a chiral cation strategy is employed to construct the CPP Pt(II) complexes R/S-ABA·[Pt(ppy)Cl2] and R/S-MBA·[Pt(ppy)Cl2] through a simple one-step reaction with almost 100% yield. The circular dichroism and CPL spectra confirm that the chirality was successfully transferred to the [Pt(ppy)Cl2]- anion. The luminescence asymmetry factors (glum) are +1.4/-1.8 × 10-3 for R/S-ABA·[Pt(ppy)Cl2] and +4.4/-2.8 × 10-3 for R/S-MBA·[Pt(ppy)Cl2]. The stronger chiroptical property of R/S-MBA·[Pt(ppy)Cl2] is attributed to the enhanced chiral structural deformation and better matched electric and magnetic transition dipole moments. This chiral cation strategy is confirmed to efficiently construct CPP Pt(II) complexes, which will accelerate the development of CPP emitters towards commercialization.

2.
J Phys Chem Lett ; : 9844-9851, 2024 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-39298330

RESUMO

High-performance circularly polarized luminescent (CPL) materials have received wide attention recently by virtue of broad application in circularly polarized light-emitting diodes, 3D display, and encryption. Reaching both high luminescence efficiency and strong luminescence dissymmetry factor (glum) is still a challenging goal that requires continuous efforts. Herein, we performed a systematic theoretical investigation on the chiroptical properties of helical cylindrical molecules (-)-[4]cyclo-2,6-anthracene [(-)-[4]CA2,6] and (P)-[4]cyclo-2,8-chrysenylene [(P)-[4]CC2,8], and found that the unique and symmetric cylindrical structure could make the transition dipole moment components offset along the cylindrical surface but concentrated along the vertical central axis. This structural superiority contributes the collinear electric and magnetic transition dipole moment vectors and thus the large glum. Based on the results of decomposed transition dipole moment vectors to individual atoms, an effective strategy to enhance the glum through introducing intramolecular short-range charge transfer by embedding B,N atoms is proposed. The decreased electric transition dipole moment and well-kept magnetic transition dipole moment enable the glum of B,N-embedded designed molecules (-)-[4]CA2,6-4BN and (P)-[4]CC2,8-4BN up to -0.31 and -0.56, respectively. This molecular-insight investigation deepens the understanding of the structure-property relationship and provides efficient guidance for improving glum of CPL materials.

3.
Inorg Chem ; 63(38): 17435-17448, 2024 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-39231304

RESUMO

The photophysical properties and luminescent mechanism of a series of tripod-type Cu(I) complexes in solution and solids were comprehensively investigated through theoretical simulations. From a microscopic perspective, the experimental phenomenon is explained: (1) The intrinsic reason for the quenching of complex 1 in solution was attributed to the significant nonradiative transition caused by structural deformation; (2) In the solid, the reduced ΔEST for complex 2 effectively facilitate reverse intersystem crossing (RISC) and improves its luminescence efficiency; (3) The enhanced performance of complex 3 in solution is attributed to that its stronger steric hindrance is advantageous to decrease not only the ΔEST but also the reorganization energy through intramolecular weak interactions. Based on complex 3, the tert-butyl substituted isomeric complex 4 was designed. Complex 4 further amplifies the advantages of 3 to further promote the RISC to make full use of excitons. Meanwhile, it has an emission wavelength of 462.6 nm, which makes it an excellent candidate for high-efficiency deep-blue TADF materials. This study provides valuable information for obtaining efficient blue phosphorescence and TADF dual-channel luminescent materials.

4.
Chem Sci ; 2024 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-39144464

RESUMO

Organic photothermal materials based on conjugated structures have significant potential applications in areas such as biomedical diagnosis, therapy, and energy conversion. Improving their photothermal conversion efficiency through molecular design is critical to promote their practical applications. Especially in similar structures, understanding how the position of heteroatoms affects the conversion efficiency is highly desirable. Herein, we prepared two isomeric small D-A molecules with different sulfur atom positions (TBP-MPA and i-TBP-MPA), which display strong and broad absorption in the UV-visible region due to their strong intramolecular charge transfer characteristics. Compared to i-TBP-MPA, TBP-MPA demonstrates aggregation-induced photothermal enhancement (AIPE). Under simulated sunlight (1 kW m-2) irradiation, the stable temperature of TBP-MPA powder reached 60 °C, significantly higher than the 50 °C achieved by i-TBP-MPA. Experimental and theoretical results indicate that the S⋯N non-covalent interactions in TBP-MPA impart a more rigid conjugated framework to the molecule, inducing ordered molecular stacking during aggregation. This ordered stacking provides additional non-radiative transition channels between TBP-MPA molecules, enhancing their photothermal performance in the aggregated state. Under 1 sun irradiation, TBP-MPA achieved a water evaporation rate of 1.0 kg m-2 h-1, surpassing i-TBP-MPA's rate of 0.92 kg m-2 h-1.

5.
J Hazard Mater ; 478: 135509, 2024 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-39167927

RESUMO

Developing high-temperature-resistant adsorbents with superior porous properties is crucial for safely disposing of heavy metal-containing solid waste via pyrolysis. We synthesized aluminosilicates hydrothermally and observed that acidic conditions, especially HCl (pH=2.6), favored sponge-like mineral (NC2.6) formation with a specific surface area of 500.31 m²/g and pore volume of 0.986 cm³ /g, while alkaline conditions (pH=12.0) promoted spherical particle growth. NC2.6 exhibited higher adsorption capacity compared to kaolinite and halloysite in the PbCl2 vapor adsorption, reaching a maximum of 137.68 mg/g at 700 â„ƒ (75.91 % stable). We examined the effect of CO2 and H2O on adsorption efficiency and explored the mechanisms using DFT and GCMC simulations. From GCMC results, CO2 negatively impacted PbCl2 adsorption due to competitive adsorption, while H2O increased adsorption content (144.24 mg/g at 700 â„ƒ) by converting PbCl2 into oxides. DFT revealed the presence of CO2 enhanced the adsorption stability of PbCl2 via the formation of covalent bonds between O in CO2 and Pb, and active O on the aluminosilicate surface. H2O increased PbCl2 adsorption energy, as O in H2O occupied an active Al that originally formed a covalent bond with Cl, while the H formed a weak hydrogen bond with this Cl.

6.
Angew Chem Int Ed Engl ; 63(34): e202407355, 2024 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-38837587

RESUMO

The structure of molecular aggregates is crucial for charge transport and photovoltaic performance in organic solar cells (OSCs). Herein, the intermolecular interactions and aggregated structures of nonfused-ring electron acceptors (NFREAs) are precisely regulated through a halogen transposition strategy, resulting in a noteworthy transformation from a 2D-layered structure to a 3D-interconnected packing network. Based on the 3D electron transport pathway, the binary and ternary devices deliver outstanding power conversion efficiencies (PCEs) of 17.46 % and 18.24 %, respectively, marking the highest value for NFREA-based OSCs.

7.
J Control Release ; 370: 866-878, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38685386

RESUMO

Glioblastoma (GBM) as one of the most lethal brain tumours, remains poor therapeutic index due to its typical characters including heterogeneous, severe immune suppression as well as the existence of blood brain barrier (BBB). Immune sonodynamic (ISD) therapy combines noninvasive sonodynamic therapy with immunotherapy, which has great prospects for the combinational treatment of GBM. Herein, we develop macrophage cell membrane cloaked reactive oxygen species (ROS) responsive biomimetic nanoparticles, co-delivering of sonosensitizer Ce6 and JQ1 (a bromo-domain protein 4 (BRD4) inhibitor which can down-regulate PD-L1) and realizing potent GBM ISD therapy. The ApoE peptide decorated macrophage membrane coating endows these biomimetic nanoparticles with low immunogenicity, efficient BBB permeability, prolonged blood circulation half-live and good biocompatibility. The ROS responsive polymeric inner core could be readily degraded as triggered by excessive ROS under the ultrasound once they accumulated in tumour cells, fast release encapsulated drugs. The generation of ROS not only killed tumour cells via sonodynamic therapy, but also induced immunogenic cell death (ICD) and further activated the anti-tumour immune response. The released JQ1 inhibited tumour cell proliferation and augmented the immune activities by inhibiting the PD-L1 expression on the surface of tumour cells. The cascade sonodynamic and immune therapy resulted in significantly improved median survival time in both orthotopic GL261 and PTEN deficient immunosuppressive CT2A GBM mice models. Therefore, our developed biomimetic nanoparticle platform provides a promising combinational therapy strategy to treat immune suppressive GBM.


Assuntos
Neoplasias Encefálicas , Glioblastoma , Macrófagos , Nanopartículas , Espécies Reativas de Oxigênio , Triazóis , Terapia por Ultrassom , Glioblastoma/terapia , Glioblastoma/tratamento farmacológico , Glioblastoma/imunologia , Animais , Terapia por Ultrassom/métodos , Humanos , Espécies Reativas de Oxigênio/metabolismo , Linhagem Celular Tumoral , Neoplasias Encefálicas/terapia , Neoplasias Encefálicas/tratamento farmacológico , Neoplasias Encefálicas/imunologia , Macrófagos/efeitos dos fármacos , Macrófagos/imunologia , Nanopartículas/química , Triazóis/administração & dosagem , Triazóis/química , Triazóis/farmacologia , Membrana Celular/metabolismo , Imunoterapia/métodos , Camundongos , Azepinas/administração & dosagem , Azepinas/farmacologia , Azepinas/química , Nanomedicina/métodos , Materiais Biomiméticos/química , Feminino , Antineoplásicos/administração & dosagem , Antineoplásicos/farmacologia , Antineoplásicos/uso terapêutico , Barreira Hematoencefálica/metabolismo
8.
Dalton Trans ; 53(17): 7384-7396, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38587258

RESUMO

The synthesis of nanosized ZSM-5 zeolites with high crystallinity and suitable acidity is very significant for their great potential in various catalytic applications. Herein, a series of zeolite ZSM-5 crystals with different particle sizes and SiO2/Al2O3 ratios (10-30) were synthesized by a temperature-varying two-step crystallization method in a concentrated gel system containing L-lysine and/or polyvinylpyrrolidone (PVP) additives. By optimizing the addition amounts of the two additives, the crystal size of the ZSM-5 zeolite could be reduced to less than 100 nm. Meanwhile, relatively high crystallinity and framework Al incorporation rates could be achieved, resulting in the generation of high-quality ZSM-5 nanocrystals. The nanosized H-form ZSM-5 zeolite with a SiO2/Al2O3 ratio of 20 showed enhanced catalytic efficiency and stability for the alkylation of 2-methylnaphthalene (2-MN) with methanol to produce an important intermediate, 2,6-dimethylnaphthalene (2,6-DMN). A relatively high and steady yield of 2,6-DMN (above 7.2%) could be achieved during 20 h time-on-stream at 400 °C. The smaller crystal size, higher crystallinity and framework Al content could provide more accessible Brønsted acid sites in the 10-membered ring channel of the ZSM-5 nanocrystals, which are the main active sites responsible for the shape-selectivity of the targeted product of 2,6-DMN. As a result, the formation of other side products like 1-MN and poly-MN could be effectively inhibited, thus leading to an improved 2,6-DMN yield and coke resistance over the nanosized ZSM-5 catalyst.

9.
Small ; 20(24): e2311561, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38546001

RESUMO

Balancing the rigid backbones and flexible side chains of light-harvesting materials is crucially important to reach optimized intermolecular packing, micromorphology, and thus photovoltaic performance of organic solar cells (OSCs). Herein, based on a distinctive CH-series acceptor platform with 2D conjugation extended backbones, a series of nonfullerene acceptors (CH-6F-Cn) are synthesized by delicately tuning the lengths of flexible side chains from n-octyl to n-amyl. A systemic investigation has revealed that the variation of the side chain's length can not only modulate intermolecular packing modes and crystallinity but also dramatically improve the micromorphology of the active layer and eventual photovoltaic parameters of OSCs. Consequently, the highest PCE of 18.73% can be achieved by OSCs employing D18:PM6:CH-6F-C8 as light-harvesting materials.

10.
Small ; 20(32): e2401054, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38488748

RESUMO

2D conjugated extension on central units of small molecular acceptors (SMAs) has gained great successes in reaching the state-of-the-art organic photovoltaics. Whereas the limit size of 2D central planes and their dominant role in constructing 3D intermolecular packing networks are still elusive. Thus, by exploring a series of SMAs with gradually enlarged central planes, it is demonstrated that, at both single molecular and aggerated levels, there is an unexpected blue-shift for their film absorption but preferable reorganization energies, exciton lifetimes and binding energies with central planes enlarging, especially when comparing to their Y6 counterpart. More importantly, the significance of well-balanced molecular packing modes involving both central and end units is first disclosed through a systematic single crystal analysis, indicating that when the ratio of central planes area/end terminals area is no more than 3 likely provides a preferred 3D intermolecular packing network of SMAs. By exploring the limit size of 2D central planes, This work indicates that the structural profiles of ideal SMAs may require suitable central unit size together with proper heteroatom replacement instead of directly overextending 2D central planes to the maximum. These results will likely provide some guidelines for future better molecular design.

11.
Adv Mater ; 36(23): e2401370, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38373399

RESUMO

Achieving desirable charge-transport highway is of vital importance for high-performance organic solar cells (OSCs). Here, it is shown how molecular packing arrangements can be regulated via tuning the alkyl-chain topology, thus resulting in a 3D network stacking and highly interconnected pathway for electron transport in a simple-structured nonfused-ring electron acceptor (NFREA) with branched alkyl side-chains. As a result, a record-breaking power conversion efficiency of 17.38% (certificated 16.59%) is achieved for NFREA-based devices, thus providing an opportunity for constructing low-cost and high-efficiency OSCs.

12.
Angew Chem Int Ed Engl ; 63(10): e202318143, 2024 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-38190621

RESUMO

In the development of high-performance organic solar cells (OSCs), the self-organization of organic semiconductors plays a crucial role. This study focuses on the precisely manipulation of molecular assemble via tuning alkyl side-chain topology in a series of low-cost nonfused-ring electron acceptors (NFREAs). Among the three NFREAs investigated, DPA-4, which possesses an asymmetric alkyl side-chain length, exhibits a tight packing in the crystal and high crystallinity in the film, contributing to improved electron mobility and favorable film morphology for DPA-4. As a result, the OSC device based on DPA-4 achieves an excellent power conversion efficiency of 16.67 %, ranking among the highest efficiencies for NFREA-based OSCs.

13.
Angew Chem Int Ed Engl ; 62(49): e202311686, 2023 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-37858963

RESUMO

Two exotic 6-cantilever small molecular platforms, characteristic of quite different molecular configurations of propeller and quasi-plane, are established by extremely two-dimensional conjugated extension. When applied in small molecular acceptors, the only two cases of CH25 and CH26 that could contain six terminals and such broad conjugated backbones have been afforded thus far, rendering featured absorptions, small reorganization and exciton binding energies. Moreover, their distinctive but completely different molecular geometries result in sharply contrasting nanoscale film morphologies. Finally, CH26 contributes to the best device efficiency of 15.41 % among acceptors with six terminals, demonstrating two pioneered yet highly promising 6-cantilever molecular innovation platforms.

14.
Angew Chem Int Ed Engl ; 62(44): e202312630, 2023 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-37704576

RESUMO

Due to the intrinsically flexible molecular skeletons and loose aggregations, organic semiconductors, like small molecular acceptors (SMAs) in organic solar cells (OSCs), greatly suffer from larger structural/packing disorders and weaker intermolecular interactions comparing to their inorganic counterparts, further leading to hindered exciton diffusion/dissociation and charge carrier migration in resulting OSCs. To overcome this challenge, complete peripheral fluorination was performed on basis of a two-dimensional (2D) conjugation extended molecular platform of CH-series SMAs, rendering an acceptor of CH8F with eight fluorine atoms surrounding the molecular backbone. Benefitting from the broad 2D backbone, more importantly, strengthened fluorine-induced secondary interactions, CH8F and its D18 blends afford much enhanced and more ordered molecular packings accompanying with enlarged dielectric constants, reduced exciton binding energies and more obvious fibrillary networks comparing to CH6F controls. Consequently, D18:CH8F-based OSCs reached an excellent efficiency of 18.80 %, much better than that of 17.91 % for CH6F-based ones. More excitingly, by employing D18-Cl that possesses a highly similar structure to D18 as a third component, the highest efficiency of 19.28 % for CH-series SMAs-based OSCs has been achieved so far. Our work demonstrates the dramatical structural multiformity of CH-series SMAs, meanwhile, their high potential for constructing record-breaking OSCs through peripheral fine-tuning.

15.
Antioxidants (Basel) ; 12(9)2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37760076

RESUMO

This study aimed to investigate the effects of dietary tannic acid (TAN) on the gas production, growth performance, antioxidant capacity, rumen microflora, and fermentation function of beef cattle through in vitro and in vivo experiments. TAN was evaluated at 0.15% (dry matter basis, DM) in the in vitro experiment and 0.20% (DM basis) in the animal feeding experiment. The in vitro results revealed that compared with control (CON, basal diet without TAN), the addition of TAN significantly increased the cumulative gas production and asymptotic gas production per 0.20 g dry matter substrate (p < 0.01), with a tendency to reduce methane concentration after 96 h of fermentation (p = 0.10). Furthermore, TAN supplementation significantly suppressed the relative abundance of Methanosphaera and Methanobacteriaceae in the fermentation fluid (LDA > 2.50, p < 0.05). The in vivo experiment showed that compared with CON, the dietary TAN significantly improved average daily gain (+0.15 kg/d), dressing percent (+1.30%), net meat percentage (+1.60%), and serum glucose concentration (+23.35%) of beef cattle (p < 0.05), while it also significantly reduced hepatic malondialdehyde contents by 25.69% (p = 0.02). Moreover, the TAN group showed significantly higher alpha diversity (p < 0.05) and increased relative abundance of Ruminococcus and Saccharomonas (LDA > 2.50, p < 0.05), while the relative abundance of Prevotellaceae in rumen microbial community was significantly decreased (p < 0.05) as compared to that of the CON group. In conclusion, the dietary supplementation of TAN could improve the growth and slaughter performance and health status of beef cattle, and these favorable effects might be attributed to its ability to alleviate liver lipid peroxidation, enhance glucose metabolism, and promote a balanced rumen microbiota for optimal fermentation.

16.
Metabolites ; 13(9)2023 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-37755275

RESUMO

This study explored the effects of drinking heated water in the cold seasons on the serum metabolism, rumen microbial fermentation, and metabolome of beef cattle. Twelve fattening cattle (642 ± 14.6 kg) aged 21 to 22 months were randomly and equally divided into two groups based on body weight: one receiving room-temperature water (RTW; average 4.39 ± 2.55 °C) and the other heated water (HW; average 26.3 ± 1.70 °C). The HW group displayed a significant decrease in serum glucose (p < 0.01) and non-esterified fatty acid (p < 0.01), but increases in insulin (p = 0.04) and high-density lipoprotein (p = 0.03). The rumen fermentation parameters of the HW group showed substantial elevations in acetate (p = 0.04), propionate (p < 0.01), isobutyrate (p = 0.02), and total volatile fatty acids (p < 0.01). Distinct bacterial composition differences were found between RTW and HW at the operational taxonomic unit (OTU) level (R = 0.20, p = 0.01). Compared to RTW, the HW mainly had a higher relative abundance of Firmicutes (p = 0.07) at the phylum level and had a lower abundance of Prevotella (p < 0.01), norank_f_p-215-o5 (p = 0.03), and a higher abundance of NK4A214_group (p = 0.01) and Lachnospiraceae_NK3A20_group (p = 0.05) at the genus level. In addition, NK4A214_group and Lachnospiraceae_NK3A20_group were significantly positively correlated with the rumen propionate and isovalerate (r > 0.63, p < 0.05). Prevotella was negatively correlated with rumen propionate and total volatile fatty acids (r = -0.61, p < 0.05). In terms of the main differential metabolites, compared to the RTW group, the expression of Cynaroside A, N-acetyl-L-glutamic acid, N-acetyl-L-glutamate-5-semialdehyde, and Pantothenic acid was significantly upregulated in HW. The differentially regulated metabolic pathways were primarily enriched in nitrogen metabolism, arginine biosynthesis, and linoleic acid metabolism. Prevotella was significantly positively correlated with suberic acid and [6]-Gingerdiol 3,5-diacetate (r > 0.59, p < 0.05) and was negatively correlated with Pantothenic acid and isoleucyl-aspartate (r < -0.65, p < 0.05). NK4A214_group was positively correlated with L-Methionine and glycylproline (r > 0.57, p < 0.05). Overall, our research demonstrates the important relationship between drinking water temperature and metabolic and physiological responses in beef cattle. Heating drinking water during cold seasons plays a pivotal role in modulating internal energy processes. These findings underscore the potential benefits of using heated water as a strategic approach to optimize energy utilization in beef cattle during the cold seasons.

17.
Antioxidants (Basel) ; 12(8)2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37627487

RESUMO

The research aimed to investigate the suitable drinking water temperature in winter and its effect on the growth performance, antioxidant capacity, and rumen fermentation function of beef cattle. A total of 40 beef cattle (640 ± 19.2 kg) were randomly divided into five treatments with eight cattle in each treatment raised in one pen according to initial body weight. Each treatment differed only in the temperature of drinking water, including the room-temperature water and four different heat water groups named RTW, HW_1, HW_2, HW_3, and HW_4. The measured water temperatures were 4.39 ± 2.546 °C, 10.6 ± 1.29 °C, 18.6 ± 1.52 °C, 26.3 ± 1.70 °C, and 32.5 ± 2.62 °C, respectively. The average daily gain (ADG) showed a significant linear increase during d 0 to 60 and a quadratic increase during d 31 to 60 with rising water temperature (p < 0.05), and the highest ADG of 1.1911 kg/d was calculated at a water temperature of 23.98 °C (R2 = 0.898). The average rectal temperature on d 30 (p = 0.01) and neutral detergent fiber digestibility (p < 0.01) increased linearly with increasing water temperature. Additionally, HW_2 reduced serum triiodothyronine, thyroxine, and malondialdehyde (p < 0.05), and increased serum total antioxidant capacity (p < 0.05) compared with RTW. Compared with HW_2, RTW had unfavorable effects on ruminal propionate, total volatile fatty acids, and cellulase concentrations (p < 0.05), and lower relative mRNA expression levels of claudin-4 (p < 0.01), occludin (p = 0.02), and zonula occludens-1 (p = 0.01) in the ruminal epithelium. Furthermore, RTW had a higher abundance of Prevotella (p = 0.04), Succinivibrionaceae_UCG-002 (p = 0.03), and Lachnospiraceae_UCG-004 (p = 0.03), and a lower abundance of Bifidobacteriaceae (p < 0.01) and Marinilabiliaceae (p = 0.05) in rumen compared to HW_2. Taken together, heated drinking water in cold climates could positively impact the growth performance, nutrient digestibility, antioxidant capacity, and rumen fermentation function of beef cattle. The optimal water temperature for maximizing ADG was calculated to be 23.98 °C under our conditions. Ruminal propionate and its producing bacteria including Prevotella, Succinivibrionaceae, and Lachnospiraceae might be important regulators of rumen fermentation of beef cattle drinking RTW under cold conditions.

18.
Microorganisms ; 11(8)2023 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-37630652

RESUMO

Yaks live in the harsh environment of the Qinghai-Tibet Plateau, and the cold climate causes lower growth efficiency. The aim of this experiment was to explore the effects of drinking warm water on the growth performance in yak calves and investigate the underlying physiological mechanisms. A total of 24 Datong yak calves were selected and randomly assigned into the cold water group (group C, water temperature around 0-10 °C without any heating; 58.03 ± 3.111 kg) and the warm water group (group W, water constantly heated at 2 °C; 59.62 ± 2.771 kg). After the 60-day experiment, body weight was measured, and rumen fluid and blood serum samples were collected for analysis. The results show that the body weight and average daily gain of yaks that drank warm water were higher compared to those that drank cold water (p < 0.05). The acetic, propionic, isobutyric, valeric, and isovaleric acid concentrations were higher in group W than in group C (p < 0.05). Additionally, warm water changed the ruminal microbes at different levels. At the phylum level, the relative abundance of Tenericutes, Kiritimatiellaeota, and Elusimicrobiota was higher in group C (p < 0.05). At the genus level, three genera were increased by warm water, including Ruminococcoides and Eubacteriales Family XIII. Incertae Sedis, and 12 genera were decreased, including Ruminococcus (p < 0.05). At the species level, unclassified Prevotellaceae and Ruminococcoides bili were increased by warm water compared to cold water (p < 0.05). According to the metabolomics results, metabolites, including valine, isoleucine, PC (15:0/22:2(13Z,16Z)), and LysoPC (18:0/0:0), were increased in the warm water group compared to the cold water group (p < 0.05), and were enriched in glycerophospholipid and amino acid metabolism pathways. This study analyzed the differences in ruminal microbes and metabolomes of yak calves provided with water at different temperatures and revealed the potential mechanism for better performance promoted by warm drinking water.

19.
Angew Chem Int Ed Engl ; 62(41): e202309600, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37610865

RESUMO

Due to the pronounced anisotropic response to circularly polarized light, chiral hybrid organic-inorganic metal halides have been regarded as promising candidates for the application in nonlinear chiroptics, especially for the second-harmonic generation circular dichroism (SHG-CD) effect. However, designing novel lead-free chiral hybrid metal halides with large anisotropy factors and high laser-induced damage thresholds (LDT) of SHG-CD remains challenging. Herein, we develop the first chiral hybrid germanium halide, (R/S-NEA)3 Ge2 I7 ⋅H2 O (R/S-NGI), and systematically investigated its linear and nonlinear chiroptical properties. S-NGI and R-NGI exhibit large anisotropy factors (gSHG-CD ) of 0.45 and 0.48, respectively, along with a high LDT of 38.46 GW/cm2 ; these anisotropy factors were the highest values among the reported lead-free chiral hybrid metal halides. Moreover, the effective second-order nonlinear optical coefficient of S-NGI could reach up to 0.86 pm/V, which was 2.9 times higher than that of commercial Y-cut quartz. Our findings facilitate a new avenue toward lead-free chiral hybrid metal halides, and their implementation in nonlinear chiroptical applications.

20.
Nat Commun ; 14(1): 4707, 2023 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-37543678

RESUMO

Given that bromine possesses similar properties but extra merits of easily synthesizing and polarizing comparing to homomorphic fluorine and chlorine, it is quite surprising very rare high-performance brominated small molecule acceptors have been reported. This may be caused by undesirable film morphologies stemming from relatively larger steric hindrance and excessive crystallinity of bromides. To maximize the advantages of bromides while circumventing weaknesses, three acceptors (CH20, CH21 and CH22) are constructed with stepwise brominating on central units rather than conventional end groups, thus enhancing intermolecular packing, crystallinity and dielectric constant of them without damaging the favorable intermolecular packing through end groups. Consequently, PM6:CH22-based binary organic solar cells render the highest efficiency of 19.06% for brominated acceptors, more excitingly, a record-breaking efficiency of 15.70% when further thickening active layers to ~500 nm. By exhibiting such a rare high-performance brominated acceptor, our work highlights the great potential for achieving record-breaking organic solar cells through delicately brominating.

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